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A hybridized local and charge transfer excited state for solution-processed non-doped green electroluminescence based on oligo(p-phenyleneethynylene)

Usta, Hakan; Alimli, Dilek; Ozdemir, Resul; Tekin, Emine; Alkan, Fahri; Kacar, Rifat; Altas, Ahu Galen; Dabak, Salih; Gurek, Ayse Gul; Mutlugun, Evren; Yazici, Ahmet Faruk; Can, Ayse


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      {
        "affiliation": "Abdullah Gul Univ, Dept Mat Sci & Nanotechnol Engn, TR-38080 Kayseri, Turkey", 
        "name": "Usta, Hakan"
      }, 
      {
        "affiliation": "Gebze Tech Univ, Dept Chem, TR-41400 Kocaeli, Turkey", 
        "name": "Alimli, Dilek"
      }, 
      {
        "affiliation": "Abdullah Gul Univ, Dept Mat Sci & Nanotechnol Engn, TR-38080 Kayseri, Turkey", 
        "name": "Ozdemir, Resul"
      }, 
      {
        "affiliation": "Sci & Technol Res Council Turkey TUBITAK, Marmara Res Ctr MAM, TR-41470 Kocaeli, Turkey", 
        "name": "Tekin, Emine"
      }, 
      {
        "affiliation": "Abdullah Gul Univ, Dept Mat Sci & Nanotechnol Engn, TR-38080 Kayseri, Turkey", 
        "name": "Alkan, Fahri"
      }, 
      {
        "affiliation": "Sci & Technol Res Council Turkey TUBITAK, Marmara Res Ctr MAM, TR-41470 Kocaeli, Turkey", 
        "name": "Kacar, Rifat"
      }, 
      {
        "affiliation": "Sci & Technol Res Council Turkey TUBITAK, Marmara Res Ctr MAM, TR-41470 Kocaeli, Turkey", 
        "name": "Altas, Ahu Galen"
      }, 
      {
        "affiliation": "Sci & Technol Res Council Turkey TUBITAK, Marmara Res Ctr MAM, TR-41470 Kocaeli, Turkey", 
        "name": "Dabak, Salih"
      }, 
      {
        "affiliation": "Gebze Tech Univ, Dept Chem, TR-41400 Kocaeli, Turkey", 
        "name": "Gurek, Ayse Gul"
      }, 
      {
        "affiliation": "Abdullah Gul Univ, Dept Elect & Elect Engn, TR-38080 Kayseri, Turkey", 
        "name": "Mutlugun, Evren"
      }, 
      {
        "affiliation": "Abdullah Gul Univ, Dept Mat Sci & Nanotechnol Engn, TR-38080 Kayseri, Turkey", 
        "name": "Yazici, Ahmet Faruk"
      }, 
      {
        "affiliation": "Abdullah Gul Univ, Dept Mat Sci & Nanotechnol Engn, TR-38080 Kayseri, Turkey", 
        "name": "Can, Ayse"
      }
    ], 
    "description": "We herein report a new highly efficient green emissive hot-exciton molecule, 1,4-bis((4'-diphenylamino3-cyano-[1,1'-biphenyl]-4-yl)ethynyl)-2,5-bis(2-ethylhexyloxy)benzene (2EHO-TPA-CNPE) that consists of an extended D'-pi'-A-pi-D-pi-A-pi'-D' molecular p-system with diphenylamino end units (D') and ethynylene/phenylene spacers (pi/pi'). The new molecule exhibits high photoluminescence (PL) quantum efficiencies (Phi(PL) = 0.95 (solution) and 0.45 (spin-coated neat thin-film)), and a strong PL solvatochromic behavior revealing significant changes in excited state energies/characteristics (locally excited (LE) -> hybridized local and charge transfer (HLCT) - charge-transfer (CT)) depending on solvent polarity. Highly efficient (radiative exciton yield (eta(r)) = 50-59% >> 25%) green-emitting OLEDs were fabricated in a conventional device architecture by employing (non-)doped thin-films reaching a maximum current efficiency (CEmax) of 12.0 cd A(-1) and a maximum external quantum efficiency (EQE(max)) of 5.5%. The emission profile of the non-doped OLED has CIE 1976 (u', v') chromaticity coordinates of (0.10, 0.55) corresponding to a night vision imaging system (NVIS) compatible Green A region. 2EHO-TPA-CNPE-based OLED devices of industrial relevance were also fabricated by ink-jet printing the emissive layer and by fabricating an inverted architecture, which possessed respectable device performances of 2.4-6.1 cd A(-1). The solid-state solvation effect in OLED devices yields HLCT electronic behavior resulting in high Zr's, which is confirmed by TDDFT to originate from energetically/spatially favorable reverse intersystem crossings (RISCs) (T-2/3 -> S-1). As a unique observation, delayed fluorescence due to this RISC was evident in the PL decay lifetime measurement with a ns-scale lifetime of similar to 10 ns. These results clearly allow a better understanding of the structure-photophysical property-electroluminescence relationships in this new class of oligo(p-phenyleneethynylene)-based hot-exciton molecules, and it could open up new opportunities for high-performance solution-processed optoelectronic/sensing applications.", 
    "doi": "10.1039/d0tc01266a", 
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    "journal": {
      "issue": "24", 
      "pages": "8047-8060", 
      "title": "JOURNAL OF MATERIALS CHEMISTRY C", 
      "volume": "8"
    }, 
    "license": {
      "id": "cc-by"
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    "publication_date": "2020-01-01", 
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    "title": "A hybridized local and charge transfer excited state for solution-processed non-doped green electroluminescence based on oligo(p-phenyleneethynylene)"
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